Methanol to propylene: Effect of phosphorus on a high silica HZSM-5 catalyst

Liu, Jian; Zhang, Chenxi; Shen, Zhenhao; Hua, Weiming; Tang, Yi; Shen, Wei; Yue, Yinghong; Xu, Hualong

doi:10.1016/j.catcom.2009.04.004

Cited by 196 publications

(125 citation statements)

References 25 publications

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“…However, improved olefin and especially propylene selectivity can be achieved using highly siliceous H-ZSM-5. 5,6 The selectivity towards propylene is increased even more with the introduction of phosphorus. [6][7][8][9][10] Usually, the improved selectivity towards propylene is attributed to the decrease in the acid site strength that is so often observed in phosphated H-ZSM-5, although steric factors have also been suggested to be responsible.…”

Section: Introductionmentioning

confidence: 99%

“…5,6 The selectivity towards propylene is increased even more with the introduction of phosphorus. [6][7][8][9][10] Usually, the improved selectivity towards propylene is attributed to the decrease in the acid site strength that is so often observed in phosphated H-ZSM-5, although steric factors have also been suggested to be responsible. [6][7][8][9][10][11][12] Even though there is still some debate on the effect of acid site strength on the MTO product distribution, the promoting effect of phosphorus on the hydrothermal stability of H-ZSM-5 is undisputed.…”

Section: Introductionmentioning

confidence: 99%

“…[6][7][8][9][10] Usually, the improved selectivity towards propylene is attributed to the decrease in the acid site strength that is so often observed in phosphated H-ZSM-5, although steric factors have also been suggested to be responsible. [6][7][8][9][10][11][12] Even though there is still some debate on the effect of acid site strength on the MTO product distribution, the promoting effect of phosphorus on the hydrothermal stability of H-ZSM-5 is undisputed. 4,9,[13][14][15][16][17][18][19][20][21][22][23][24][25] Zeolite H-ZSM-5 catalysts that contain phosphorus are more stable under hydrothermal conditions i.e.…”

Section: Introductionmentioning

confidence: 99%

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Local silico-aluminophosphate interfaces within phosphated H-ZSM-5 zeolites

Bij

Weckhuysen

2014

Phys. Chem. Chem. Phys.

127

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In order to elucidate phosphorus-zeolite H-ZSM-5 interactions, a variety of phosphorus-modified zeolite H-ZSM-5 materials were studied in a multi-spectroscopic manner. By deploying single pulse 27 Al, 31 P MAS NMR, 2D heteronuclear 27 Al-31 P correlation (HETCOR), 27 Al MQ MAS NMR spectroscopy, TPD of pyridine monitored by FT-IR spectroscopy, and Scanning Transmission X-ray Microscopy (STXM) the interplay and influence of acidity, thermal treatment and phosphorus on the structure and acidity of H-ZSM-5 were established. It was found that while acid treatment did not affect the zeolite structure, thermal treatment leads to the breaking of Si-OH-Al bonds, a decrease in the strong acid site number and the formation of terminal Al-OH groups. No extra-framework aluminium species was observed. Phosphorus precursors interact with the zeolitic framework through hydrogen bonds and physical coordination, as phosphorus species can be simply washed out with hot water. After phosphatation and thermal treatment two effects occur simultaneously, namely (i) phosphorus species transform into water insoluble condensed poly-phosphoric acid and (ii) phosphoric acid binds irreversibly to the terminal Al-OH groups of partially dislodged four-coordinated framework aluminium, forming local silico-aluminophosphate interfaces.These interfaces are potentially the promoters of hydrothermal stability in phosphated zeolite H-ZSM-5.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Local silico-aluminophosphate interfaces within phosphated H-ZSM-5 zeolites

Bij

Weckhuysen

2014

Phys. Chem. Chem. Phys.

127

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“…The acidity of catalyst plays an important role in catalytic activity through MTO reaction, and acid adjustment is the most significant affecting factor for product distribution and catalytic stability [10][11][12][13][14][15][16][17][18]. Many methods could adjust the catalysts acid properties for a better catalytic performance.…”

Section: Introductionmentioning

confidence: 99%

Effect of magnesium modification over H-ZSM-5 in methanol to propylene reaction

et al. 2015

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H-ZSM-5-based catalyst is a recognized catalyst which is particularly selective towards the formations of light olefins in the methanol reaction. A series of H-ZSM-5 (SiO 2 /Al 2 O 3 = 38) modified with different amounts of magnesium have been investigated. All the samples were characterized by X-ray diffraction instrument (XRD), temperature-programmed desorption of NH 3 (NH 3 -TPD) and Fourier Transform Infrared Spectoscopy (FT-IR). The results indicated that the impregnation of H-ZSM-5 (SiO 2 /Al 2 O 3 = 38) zeolite with various magnesium loading amount significantly affected the strength of acid sites and decreased the concentration of both weak and strong acid sites. As a result of modification, magnesium mainly interacted with strong Brønsted acid sites, thus generated new medium strong acid sites and enhanced the yield of propylene. The optimum acid property for methanol to propylene (MTP) reaction was gotten over 4.0 Mg-ZSM-5 (4.0 wt% Mg) zeolite catalyst. The maximum yield of propylene was 10.62 wt% over 4.0 Mg-ZSM-5 zeolite catalyst by the 30 min on stream. Coke which was mostly formed on strong Brønsted acid sites, would cause the catalysts deactivation, so the reduction of strong Brønsted acid sites could enhance the catalytic stability.

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“…Especially for propylene, due to the growing demands and the shortage of petroleum resource in the future, new processes with a high yield of pro pylene are required. Methanol to propylene (MTP) process as the process with high yield of propylene is a promising way for the production of propylene instead of petroleum route, since methanol can be easily produced from natural gas and coal [1][2][3] . As compared to the methanol to olefi ns (MTO) process, where ethylene is the main product, high propylene to ethylene ratio is the most distinguishable feature for MTP that enables the high propylene yield in the recirculation process 4 .…”

Section: Introductionmentioning

confidence: 99%

Effect of boron on ZSM-5 catalyst for methanol to propylene conversion

Zhang

et al. 2013

Polish Journal of Chemical Technology

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B-ZSM-5 catalysts were prepared by various modifi cation methods with boric acid, including ion-exchange, impregnation and direct synthesis. The catalysts were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), NH 3 -Temperature Programmed Desorption (NH 3 -TPD), N 2 adsorption-desorption, Fourier Transform Infrared spectrometry (FT-IR), 27 Al and 11 B MAS NMR spectra. The results revealed that the weak acidity of catalysts was signifi cantly increased by modifi cation. The catalytic activity was measured in a fi xed bed at 460 o C for methanol to propylene (MTP) reaction. The results of MTP reaction showed a great increment of the propylene selectivity for the boron modifi ed samples, especially for the directly synthesized B-ZSM-5 which also displayed high activity and selectivity towards C 2 = -C 4 = olefi ns. It was found that the remarkable selectivity strongly depended on the intensity of weak acidity.

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Methanol to propylene: Effect of phosphorus on a high silica HZSM-5 catalyst

Cited by 196 publications

References 25 publications

Local silico-aluminophosphate interfaces within phosphated H-ZSM-5 zeolites

Local silico-aluminophosphate interfaces within phosphated H-ZSM-5 zeolites

Effect of magnesium modification over H-ZSM-5 in methanol to propylene reaction

Effect of boron on ZSM-5 catalyst for methanol to propylene conversion

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